240Pu/239Pu isotopic ratios and 239+240Pu total measurements in surface and deep waters around Mururoa and Fangataufa atolls compared with Rangiroa atoll (French Polynesia)

The average values of (240)pU/ (239)pU mass isotopic ratios of plutonium deposited in Mururoa and Fangataufa atoll sediments by French atmospheric nuclear tests range from 3.5 to 5%. In order to assess the near field and far field influence of those deposits in the open ocean, two water profiles were measured for (239+240)pU and (PU)-P-240/ (239)pU using, for the first time, an Inductively Coupled Plasma Mass Spectrometer which was developed to achieve femtogram detection limits. One site was located at the limit of the French territorial waters, which is 22 km distant from Mururoa. The second site was located close to Rangiroa atoll, at a distance of approximately 1200-km from French nuclear test sites. The sample volumes were approximately 500 litres and plutonium was purified prior to mass spectrometry and alpha spectrometry measurements. In Rangiroa, the (239+240)pU profile is comparable with those already determined in world open oceans but the maximum detected activity, 9 mBq/m(3) at 500-600 m is a lot lower than those measured in the northern hemisphere. (240)pU/ (239)pU ratios were measured between 500 and 1000 m and were not statistically different from the typical 0.18+/-0.01 ratio which characterises the global fallout. Consequently, any influence of plutonium from the tests in Mururoa and Fangataufa is not apparent at Rangiroa. The vertical distribution of 239+240pU near Mururoa shows similar changes with depth but with a slight increase in concentration. (240)pU/ (239)pU mass ratios vary with depth, from 7 to 10% in the upper 500 m and in the deep waters (below 1000 m) to 15-16% between 600 and 1000 m. A contribution from plutonium deposited in the sediments at Mururoa and Fangataufa is observed at the limit of territorial waters, especially in surface and deep waters. (C) 1999 Elsevier Science B.V. All rights reserved.